Oil preserved in fluid inclusions in quartz grains suggests hydrocarbon generation and migration occurred during the Archaean. Multiple generations of oil migration are indicated by:. Oil inclusions within early diagenetic cements at different levels in the stratigraphic succession. Oil-bearing fluid inclusions within detrital sandstone fragments suggest that oil migration also occurred in a sedimentary succession on the Kaapvaal Craton prior to 2. Ga.
Original Description:
Original Title
Archaean Oil Migration in the Wit Waters Rand Basin of South Africa
Oil preserved in fluid inclusions in quartz grains suggests hydrocarbon generation and migration occurred during the Archaean. Multiple generations of oil migration are indicated by:. Oil inclusions within early diagenetic cements at different levels in the stratigraphic succession. Oil-bearing fluid inclusions within detrital sandstone fragments suggest that oil migration also occurred in a sedimentary succession on the Kaapvaal Craton prior to 2. Ga.
Oil preserved in fluid inclusions in quartz grains suggests hydrocarbon generation and migration occurred during the Archaean. Multiple generations of oil migration are indicated by:. Oil inclusions within early diagenetic cements at different levels in the stratigraphic succession. Oil-bearing fluid inclusions within detrital sandstone fragments suggest that oil migration also occurred in a sedimentary succession on the Kaapvaal Craton prior to 2. Ga.
Journal of the Geological Society, London, Vol. 159, 2002, pp. 189201. Printed in Great Britain.
Archaean oil migration in the Witwatersrand Basin of South Africa
G. L. ENGLAND 1,2 , B. RASMUSSEN 1 , B. KRAPEZ{ 1 & D. I. GROVES 1 1 Centre for Global Metallogeny, Department of Geology and Geophysics, University of Western Australia, 35 Stirling Highway, Crawley, WA 6009, Australia 2 Present Address: Department of Geology and Geophysics, Grant Institute, University of Edinburgh, Edinburgh, EH9 3JW, UK (e-mail: Gavin.England@glg.ed.ac.uk) Abstract: The Late Archaean Witwatersrand Supergroup of South Africa hosts the largest known gold-uranium-pyrite ore deposits. Oil preserved in uid inclusions in quartz grains in siliciclastic sedimentary rocks of that supergroup implies that hydrocarbon generation and migration occurred during the Archaean, and may have been involved in mineralization processes. Through reference to Phanerozoic analogues, oil-bearing uid inclusions entrapped in healed microfractures in detrital quartz grains and in early syntaxial quartz-overgrowths imply, that the onset of oil migration coincided with early to intermediate stages of burial, while intra-granular porosity was still preserved. Multiple generations of oil migration are indicated by: (i) oil inclusions within early diagenetic cements at dierent levels in the stratigraphic succession; (ii) more than one type of oil in entrapment sites; (iii) oil entrapment in multiple stages of the quartz paragenetic sequence. Oil generation and migration are considered to have occurred throughout, and for some considerable time after, development of the Witwatersrand Basin, consistent with progressive burial and kerogen maturation in more than one tectonic regime. Oil-bearing uid inclusions within detrital sandstone fragments suggest that oil migration also occurred in a sedimentary succession on the Kaapvaal Craton prior to 2.9 Ga. Oil in the Witwatersrand Supergroup was most likely derived from multiple source areas, with the principal source probably being shales within the lower Witwatersrand Supergroup. The hydrocarbon migration history of the basin has important implications for understanding the textural relationship between gold, bituminized oil and uraninite in the giant gold-uranium-pyrite ore deposits. Keywords: Witwatersrand, gold, uraninite, hydrocarbons, uid inclusions. Conglomerate- and sandstone-hosted gold-uranium-pyrite ore deposits of the Witwatersrand in South Africa have provided nearly 40% of world gold production over the whole span of recorded history (Pretorius 1991), although previous estimates have suggested a proportion as high as 55% (Pretorius 1976). In all its statistics, whether tonnes of ore mined, tonnes of gold, uranium and even pyrite produced, depth and areal extent of mining, or number of mines, the Witwatersrand ranks unreservedly as giant and of unparalleled economic signi- cance. The ore-deposits, their host sedimentary units and the four depositional basins to those successions (Dominion, Witwatersrand, Ventersdorp, Transvaal) are also of great geological interest. Of particular interest here is that three of the successions (Witwatersrand, Ventersdorp, Transvaal) pre- serve evidence for the migration and trapping of oil during the Late Archaean. Notwithstanding the long and continuing debate on the origin of the gold, uranium and pyrite mineralization, the origin of bituminous nodules and seams within the ore deposits (or reefs), and particularly within the Late Archaean Witwatersrand Supergroup, has also long been a source of controversy (Pretorius 1991; Gray et al. 1998). Early investi- gators (e.g., Young 1917) recognized bitumen (referred to then as carbon) as having a strong spatial relationship with gold, uraninite and pyrite. There was, however no detailed research on the origin of bitumen until the 1950s and 1960s (e.g., Davidson & Bowie 1951; Liebenberg 1955; Ramdohr 1958; Snyman 1965). The two principal hypotheses on the origin of the bitumen are that it is either: (i) the fossil remains of in situ algae which colonized sediment surfaces (Snyman 1965; Hallbauer 1975; Zumberge et al. 1981; Ebert et al. 1990); or (ii) the residual product of migrating liquid hydrocarbons (Liebenberg 1955; Schidlowski 1981; Parnell 1996; Buick et al. 1998; Gray et al. 1998). While the hypothesis of a syngenetic algal residue was prominent during the 1970s and 1980s, more-recent organic-geochemical, stable-isotopic and petrographic studies (Gray et al. 1998; Robb et al. 1999; Spangenberg & Frimmel 2001) support the hypothesis that bitumen originated from migrating hydrocarbons. Bituminous nodules are interpreted to have formed by the polymerization and crosslinking of liquid hydrocarbons around irradiating detrital heavy-mineral grains (principally uraninite) in the host sedimentary rock (Liebenberg 1955; Schidlowski 1981). Although most recent studies agree that the formation of bituminous nodules in Witwatersrand (and Ventersdorp and Transvaal-Black Reef) ore deposits involved migrating hydro- carbons, the timing of oil migration and the mechanism by which oil entered reef systems remain unclear. Whereas some investigators consider that hydrocarbon migration occurred during early burial and was focused into horizons that retained primary porosity (Buick et al. 1998; England et al. 2001), others have suggested that the major conduit for oil migration was fracture-dominant secondary porosity that post-dated occlusion of primary porosity by burial quartz cementation and pressure solution (Robb et al. 1997; Gray et al. 1998; Parnell 1999). Some authors have suggested also that hydro- carbon generation and migration occurred during deposition of the Transvaal Supergroup (Robb et al. 1997; Drennan et al. 1999), some 180270 million years after deposition of the Witwatersrand Supergroup. 189 Liquid hydrocarbon inclusions have been identied recently within authigenic quartz cements in mineralized conglomerates from the Witwatersrand (Dutkiewicz et al. 1998). Similar oil-bearing uid inclusions in quartz, carbonate and feldspar cements from Phanerozoic reservoir rocks (Burruss 1981; Lisk & Eadington 1994; Parnell et al. 1998) are used commonly to constrain the timing of hydrocarbon migration relative to cement paragenesis. By analogy, this paper focuses on the petrographic and stratigraphic distribution of oil-bearing uid inclusions in the Witwatersrand Supergroup, the Ventersdorp Contact Reef at the base of the Ventersdorp Supergroup, and the Black Reef at the base of the Transvaal Supergroup. The study examines: (i) the timing and mechanisms for oil migration in the Witwatersrand Basin, in relation to both quartz cementation history and basin evolution and (ii) the relationship between oil migration and the formation of bitumen nodules and gold mineralization. The results indicate that processes of oil generation and migration, and their timing relative to burial history, have not changed since the Archaean. Geological setting The Witwatersrand Supergroup is the structural remnant of what was originally a more extensive succession deposited within the central portions of the Kaapvaal Craton of South Africa (Fig. 1). The Supergroup is an approximately 75 km thick succession of mudrock, sandstone and minor conglom- erate that was deposited some time between 309 and 271 Ga (Armstrong et al. 1991). The original Witwatersrand Basin is considered to have been similar in geotectonic setting to modern retroarc (foreland) basins (Burke et al. 1986), such as those east of the American Cordillera (e.g., Rocky Mountains and Andean Foreland Basins). According to Winter (1987), the Witwatersrand Supergroup can be divided into: (i) a lower marine-inuenced deltaic stage (West Rand Group) and (ii) an upper uviodeltaic stage (Central Rand Group). The older Dominion Group is considered to record a back-arc basin that predated the Witwatersrand Basin by at least 100 million years. The Dominion Reef, a siliciclastic succession at the base of the Dominion Group, is a uraninite-pyrite ore-deposit with low gold content. Compressive deformation associated with the Limpopo Orogeny is considered to have produced synsedimentary thrust- and wrench-faulting of the West Rand and Central Rand successions, with subsequent uplift, sediment recycling and stacking of unconformities (Coward et al. 1995). Each unconformity surface is overlain by transgressive quartz- pebble conglomerate lags and pyritic cross-bedded sandstones, which, in selected stratigraphic locations, are the host to gold and uranium ore bodies (i.e., reefs). In addition to burial and deformation related to episodic synsedimentary subsidence and uplift, several post- Witwatersrand, Archaean and Proterozoic events have modied the Witwatersrand Supergroup. These include (after Coward et al. 1995; Martin et al. 1998): (i) stacked episodes of ood- basalt volcanism, uplift, erosion and half-graben deposition of the Ventersdorp Supergroup; (ii) folding and thrusting prior to deposition of the Transvaal Supergroup; (iii) passive-margin thermal subsidence and exural reactivation during deposition of the Chuniespoort Group (lower Transvaal Supergroup); (iv) rift-basin deposition of the Duitschland Formation and Preto- ria Group (middle Transvaal Supergroup); (v) emplacement of the Bushveld Igneous Complex associated with lithospheric extension and high heat-ow, coeval with deposition of the Rooiberg Group (upper Transvaal Supergroup); (vi) strike-slip deformation associated with uplift of the Vredefort Dome. These events are linked to several phases of metamorphism and alteration, with peak metamorphism reaching lower greenschist temperatures of 350 50 C (Phillips & Law 1994). There is extensive debate as to whether major ore com- ponents (gold, uraninite, pyrite) in reefs were: (i) introduced as detrital heavy minerals and later remobilized during meta- morphism or hydrothermal alteration (Minter 1978; Frimmel 1997; Robb et al. 1997) or (ii) introduced by hydrothermal uids during metamorphism (Phillips & Myers 1989; Barnicoat et al. 1997; Phillips & Law 2000). The second hypothesis requires more than one hydrothermal event because gold- pyrite uraninite mineralization is recorded from the basal stratigraphic succession of the Ventersdorp Supergroup (Ventersdorp Contact Reef), which post-dates folding, faulting and mineralization of the Witwatersrand Supergroup (Krapez 1985), and from the basal Black Reef of the Transvaal Supergroup, which similarly post-dates the Ventersdorp Supergroup. Fig. 1. Subsurface geological map and stratigraphic column of the Witwatersrand Basin, including the localities of the Welkom (WGF), Klerksdorp (KGF) and Carletonville Goldelds (CGF): modied after Frimmel (1997). 190 G. L. ENGLAND ET AL. Methods Sampling Samples were collected of mineralized and non-mineralized sedimen- tary rocks from underground mine workings and diamond drill core on the Welkom, Klerksdorp and Carletonville Goldelds (Fig. 1). Sampled intervals include: (i) the Steyn and Leader Reefs from Freegold One (President Steyn Mine) on the Welkom Goldeld; (ii) sub-economic reefs (e.g., A and B Reefs) and uneconomic conglomer- ates, sandstones and mudrocks in the Freegold Mining Lease on the Welkom Goldeld; (iii) the Vaal and C Reefs, as well as uneconomic conglomerates, sandstones and mudrocks from Vaal Reef Numbers 8 and 9 Shaft on the Klerksdorp Goldeld; (iv) the Ventersdorp Contact and Dennys Reefs from Vaal Reef Number 10 Shaft on the Klerksdorp Goldeld; (v) the Inner Basin Reef (upper West Rand Group) from the Afrikander Lease on the Klerksdorp Goldeld; (vi) the Dominion Reef from the Dominion Lease on the Klerksdorp Goldeld; (vii) the Carbon Leader and Black Reef from Western Deep Levels on the Carletonville Goldeld; (viii) the Ventersdorp Contact Reef from Elandsrand Mine on the Carletonville Goldeld; (ix) the Black Reef, from diamond drill core, in the Potchefstroom Gap Area between the Klerksdorp and Carletonville Goldelds. UV-epiuorescent microscopy Oil-bearing uid inclusions were identied in polished thin-sections from many of the samples using conventional transmitted light (TL) and ultra-violet (UV) epiuorescence microscopy. The process in- volved the attachment of a vertical UV illuminator to a conventional TL microscope, allowing observation under long-wave UV vertical illumination (Burruss 1981). Liquid hydrocarbons, if present within uid inclusions, will uoresce under ultra-violet excitement. The various uorescent colours and intensities relate to dierences in organic chemical composition and are controlled essentially by the type and concentration of aromatic molecules (and to a lesser degree, N-, S- and O-bearing compounds), relative to aliphatic compound concentrations (Stasiuk & Snowden 1997). Various researchers that discuss oil uorescence (Hagemann & Hollerbach 1986; McLimans 1987; Bodnar 1990; Lisk & Eadington 1994) often relate variations in uorescence colours to dierences in oil gravity (API number), which may directly relate to oil maturation. Oil at the red end of the uorescent spectrum is considered to be produced from source rocks at the onset of oil generation, representing low maturity heavy oils. The blue and white uorescent colours at the other end of the spectrum represent light oil or condensate expelled from source rocks at higher levels of maturity, corresponding with peak to late generation (Lisk & Eadington 1994). This, however does not take into account other complexities, which may alter hydro- carbon composition and thus aect UV uorescence (George et al. 2001). Complexities may include: (i) variation in source rock type, although this had a less-signicant eect with Archaean oils, which could have been derived from only bacterial-algal Type I or Type II kerogens (Mossman & Tompson-Rizer 1993); (ii) oil fractionation due to water ushing and biodegradation during migration (Bodnar 1990); (ii) fractionation of oil during trapping (George et al. 2001); (iv) thermal alteration of oil during migration (Killops & Killops 1993). With little detailed information on the organic chemistry of Archaean oil, and to what extent chemical, thermal or biological interaction processes may have been involved during oil migration, it is dicult to interpret the causes for the variations in uorescence evident from samples examined during this study. Whereas some studies of Phanerozoic oil suggest that samples containing more than one uorescent colour reect multiple oil migration events or dierent sources (McLimans 1987; Eadington et al. 1991), others recommend caution because single oil charges can show dierent colour populations (George et al. 2001). SEM The uid-inclusion history derived from samples of sandstones and conglomerates of the Witwatersrand Supergroup is complex. The complexity arises not only from uid inclusions trapped during post-depositional activity, but also from uid inclusions in detrital quartz grains. In some cases, to assist in dening the paragenetic timing of oil-bearing uid-inclusion entrapment, selected polished thin-sections were examined also by cathodoluminescence scanning- electron microscopy (CL-SEM), which provides a means of identify- ing: (i) healed microfractures (evident as uid inclusion trails under TL microscopy) and (ii) secondary quartz cements, which are optically indistinguishable from detrital quartz grains in conventional optical microscopy. CL-SEM imagery of Phanerozoic sandstones is often used to distinguish detrital quartz grains from diagenetic quartz over- growths and fracture ll (Hogg et al. 1992; Sullivan et al. 1997; Milliken & Labach 2000). Detrital quartz from an igneous source is usually substantially brighter in luminescence than quartz of an authigenic origin (i.e., overgrowth and fracture ll). Oil-bearing uid inclusions: results and discussion Inclusion description Of the 62 polished thin-sections examined under UV illumi- nation during this study, 41 have uid inclusions that contain liquid hydrocarbons. The oil-bearing uid inclusions range from 3 to 15 m in diameter. They are hosted in either healed microfractures within detrital quartz grains or are primary inclusions within syntaxial quartz overgrowths (Figs 2 and 3). Although some re-equilibration of uid inclusions could have been expected due to increasing temperature and burial during basin subsidence and subsequent metamorphism (McLimans 1987), in most cases the liquid hydrocarbons within the uid inclusions are well preserved. They appear typically as three Fig. 2. Schematic diagram showing entrapment sites of uid inclusions within sandstones and conglomerates. ARCHAEAN OIL MIGRATION IN SOUTH AFRICA 191 phases (clear liquid-oil-gas bubble), although four phases (clear liquid-oil-clear liquid-gas) and oil-only inclusions are present. The oil portion of the inclusions is represented by either a clear, light or dark brown liquid rim, which typically surrounds the mobile gas phase and ranges from 5 to 20% of the total volume of each uid inclusion (Fig. 3a and b). Although some oil-bearing uid inclusions exhibit textural evidence of auto-decrepitation and necking-down, the majority show rounded or negative crystal shapes. The oil-bearing uid inclusion morphologies include spherical, oval, ellipsoidal, lath-like and irregular shapes, although there is no obvious relationship between inclusion morphology and quartz cement Fig. 3. Photomicrographs showing oil-bearing uid inclusions hosted in healed microfractures from various sandstones and conglomerates of the Witwatersrand Supergroup. (a, b) Detrital quartz grain surrounded by a matrix of sericite and brannerite (opaque) (a,TL). The quartz grain contains two large uid inclusions (marked by arrow), Vaal Reef, Klerksdorp Goldeld. A higher magnication, TL-UV composite photomicrographs (b) demonstrates that the two uid inclusions uoresce yellow-orange under UV illumination. The dark liquid rim (marked by arrows in b) surrounding the gas bubble represents the oil portion of the inclusion. (c, d) Trail of oil-bearing uid inclusions, uorescing white, green and blue (c; TL; d, UV), Leader Reef, Welkom Goldeld. (e, f) Detrital quartz grain with multiple trails of oil-bearing uid inclusions, displaying a variety of orescent colours including orange, red, yellow, green, and blue (e; TL; f, UV), Steyn Reef, Welkom Goldeld. 192 G. L. ENGLAND ET AL. history. The inclusions show a wide range of uorescent colours including red, light brown, orange, yellow, green, white and blue (Fig. 3b, d and f). Yellow is the most prominent colour recorded, and irregularly shaped inclusions are most common. Oil-bearing uid inclusions with an irregular mor- phology are generally larger than other morphological types. Petrographic distribution Fluid inclusions in samples from the Witwatersrand Supergroup, the Ventersdorp Contact Reef and the Black Reef (Fig. 2) are categorized as: (i) pre-depositional (mostly aqueous) uid inclusions hosted in detrital grains (Type 1); (ii) secondary inclusions hosted in point-contact fractures that developed during physical compaction (Type 2); (iii) primary inclusions hosted in quartz cements (Type 3); (iv) secondary inclusions hosted in deformation-related fractures (Type 4); (v) primary inclusions hosted in quartz veins (Type 5). In many cases, it can be dicult to distinguish between the various types. Resolution of some entrapment sites was achieved only by CL-SEM examination of polished thin-sections. No corre- lation was detected between entrapment site of the oil-bearing uid inclusion and UV uorescent colour. Type 1 uid inclusions are identied as those hosted in detrital quartz grains and pebbles, and in lithic fragments (e.g., rounded sandstone fragments), and that were entrapped prior to sedimentary deposition. This type, which has obvious provenance relevance, includes uid inclusions that originated in source hinterlands (Shepherd 1977; Hallbauer 1983) or in previously deposited Witwatersrand sediments that were recycled during intraformational uplift. Some inherited inclu- sions can be recognized easily within detrital quartz grains, because they are associated with microfractures and quartz- healing patterns that are dierent to those in other surround- ing framework grains. However, inherited uid inclusions in quartz pebbles and grains show no evidence of liquid hydro- carbons. The only Type 1 uid inclusions that contain oil are those hosted in rounded pebbles of sandstone. Type 2 inclusions are secondary uid inclusions hosted by healed microfractures, within detrital quartz grains (Dutkiewicz et al. 1998; Figs 2 and 4). Microfracturing, as a burial process, is considered to initiate during early stages of diagenesis (<1 km in depth; e.g., Zhang et al. 1990), but precedes the onset of pressure solution. It occurs when frame- work minerals (e.g., quartz grains) are unable to support increasing overburden. Strain, at a granular level, is taken up at grain-point contacts with resulting internal brittle failure and grain rotation (Groshong 1988; Zhang et al. 1990). Microfractures are commonly restricted to one or two grains (Groshong 1988), and typically have a wide range of orienta- tions (Borg & Maxwell 1956). In some instances, micro- fractures, when recorded under CL-SEM, can terminate at detrital grain boundaries and do not penetrate syntaxial quartz overgrowths. The healed microfractures within the detrital quartz grains that host Type 2 inclusions are texturally similar to those described by Lisk & Eadington, (1994) and Parnell et al. (1998) from Phanerozoic examples, and are similarly interpreted to be compaction-related. The microfractures are the most promi- nent textural site where oil-bearing uid inclusions were entrapped (Fig. 4), and they commonly host multiple oil- bearing uid inclusions, normally with a wide range of uo- rescent colours (Fig. 3e and f). In some cases, particular grains have been selective hosts for oil-bearing uid inclusions within point-contact fractures, perhaps due to the greater suscepti- bility of those grains to brittle failure during physical compaction. Type 3. There are liquid hydrocarbons also in primary inclusions entrapped in syntaxial quartz overgrowths (Type 3, Figs 2 and 5). Quartz cementation of siliciclastic successions can develop at moderate burial depths (1-15 km) and continue with increasing depth and temperature (Bjrlykke & Egeberg, 1993). Authigenic quartz may be derived from circulating silica-saturated pore uids or a local source such as dissolution of silicate minerals or quartz pressure solution, which initiates at moderate depths (Bjrlykke & Egeberg 1993). Although CL-SEM imagery indicates that quartz grain interpenetration was limited in Witwatersrand samples, other forms of pressure solution are evident, including extensive stylolitization and development of pressure-solution seams and zones, particularly within reef packages. Quartz appears to have been preferentially dissolved in the presence of phyllo- silicates, bitumen and heavy minerals. The oil-bearing uid inclusions hosted in quartz cements are sited typically at contacts between detrital grains and overgrowths (Fig. 5cf), implying that entrapment occurred during early cementation (cf. Lisk & Eadington 1994). Entrapment sites commonly contain multi-coloured inclusions (Fig. 5f). In many cases, quartz overgrowths were preferentially corroded and dissolved in the presence of pyrophyllite, most likely during acidic metasomatism (cf. Barnicoat et al. 1997). Type 4 uid inclusions are those entrapped in healed micro- fractures that penetrate through framework minerals and quartz cements, typically without changing fracture orien- tation. The sandstones and conglomerates must have almost fully indurated at this stage of oil migration and acted as brittle bodies. Fracturing of this nature most likely developed during multiple episodes of deformation, particularly related to post- Witwatersrand events (Coward et al. 1995). Bedding-parallel fractures associated with bitumen seams, as described by Barnicoat et al. (1997) and Gray et al. (1998), are linked to syn- to post-Witwatersrand deformation. Although those types of bedding-parallel fractures do not contain oil-bearing uid inclusions, other Type 4 sites, unrelated to bitumen seams, contain trace amounts of oil-bearing uid inclusions (e.g., C Reef, Carbon Leader Reef). These microfractures are vertical to sub-vertical in orientation, and their paragenetic timing is poorly constrained. Type 5 uid inclusions were examined also from hydro- thermal quartz veins (Type 5, Fig. 2) in the C Reef of the Klerksdorp Goldeld. These quartz veins post-date the formation of bitumen nodules hosted in the mineralized con- glomerate, and samples of veins examined during this study do not contain liquid hydrocarbons in either primary or secondary inclusions. Nevertheless, similar quartz veins sampled for uid inclusion studies by Phillips et al. (1988) and Frimmel et al. (1999) contain CH 4 , identied by a depression in the CO 2 -triple point. Any oil that was present most likely would have been coked due to higher localized uid temperature (c. 150 500 C; Drennan et al.1999) to form ARCHAEAN OIL MIGRATION IN SOUTH AFRICA 193 pyrobitumen. This may explain the presence of bitumen in inclusions hosted in quartz veins, as recorded by Drennan et al. (1999). Stratigraphic distribution Oil-bearing uid inclusions are recorded here from samples at stratigraphic intervals throughout the Central Rand Group, as Fig. 4. Photomicrographs and SEM image showing the petrographic setting of uorescent uid inclusions from Dennys Reef, Klerksdorp Goldeld. (a) TL photomicrograph shows detrital quartz grains with intra-granular pores lled with quartz and late-phase bitumen (opaque). (b) CL SEM image of (a) reveals non-luminescent quartz lling physical compaction-related microfractures and overgrowing detrital grains (indicated by arrows). (c, d) Combined TL (c) and UV (d) photomicrographs are a close up of (a) and (b) (see inserts), showing that many of the uid inclusions associated with microfractures contain oil. The oil-bearing uid inclusions in (d) uoresce yellow and light blue. 194 G. L. ENGLAND ET AL. Fig. 5. Photomicrographs and SEM images showing the petrographic setting of uorescent uid inclusions from the Steyn Reef, Welkom Goldeld. (a) TL photomicrograph showing detrital quartz grains with intra-granular pores lled with chlorite, sericite and quartz. (b) CL SEM image of (a), reveals non-luminescent quartz lling ne physical compaction-related microfractures and overgrowing detrital grains. TL photomicrograph (c) and matching CL-SEM image (d) (close up of a and b) reveal a trail of uid inclusions at the boundary between the quartz overgrowth and the detrital quartz grain (indicated by arrows). Other uid inclusion trails are conned to healed microfractures. (e, f) Fluid inclusions hosted at the overgrowth-detrital grain boundary and those conned within healed microfractures (see insert in c) show evidence of oil, indicated by green and blue uorescence under UV illumination (f). ARCHAEAN OIL MIGRATION IN SOUTH AFRICA 195 well as from samples of the Inner Basin Reef (upper West Rand Group), the Ventersdorp Contact and Black Reefs (Fig. 6). There is no obvious correlation between stratigraphic position and UV uorescent colour of oil-bearing uid inclu- sions. The oldest stratigraphic interval investigated (Dominion Reef) shows no evidence of oil-bearing uid inclusions (see also Feather & Glatthaar 1987). The implication is that the Dominion Reef most likely received no or only a minimal oil charge. Samples of the Inner Basin Reef (at the base of the Jeppestown Subgroup) contain uid inclusions with liquid hydrocarbons in Type 1 and 2 sites. Inherited oil-bearing uid inclusions (Type 1) identied in those samples are hosted in a well-cemented and partially recrystallized, rounded pebble of sandstone. Although the pebble preserves several sets of microfractures and evidence for several phases of quartz recrystallization, oil-inclusions are conned to early point- contact fractures within detrital quartz grains enclosed by Fig. 6. Stratigraphic distribution of oil-bearing uid inclusions within the Witwatersrand Supergroup, in the Welkom, Klerksdorp, and Carletonville Goldelds: stratigraphic section modied from SouthAfrican Committee for Stratigraphy (1981). Arrows indicate sections of the stratigraphic succession examined during the study. 196 G. L. ENGLAND ET AL. authigenic quartz cements. Irrespective of whether the pebble were derived intraformationally from Witwatersrand sediments or from pre-Witwatersrand source rocks, its oil- bearing uid inclusions indicate that liquid hydrocarbons migrated through sedimentary rocks before deposition of the Jeppestown Subgroup. Samples that contain oil-bearing uid inclusions come from the Central Rand Group in the Klerksdorp, Carletonville and Welkom Goldelds. The oil-lled inclusions are recorded mostly in samples from conglomerate units, particularly those that contain bituminous nodules. Oil entrapment is most prevalent in Type 2 uid inclusions, although Types 1, 3 and 4 uid inclusions are preserved also. In several cases, oil inclu- sions appear to have been entrapped at various stages in the quartz paragenetic sequence. Reefs that contain abundant oil-bearing uid inclusions, as well as bituminous nodules, are the Vaal, C and Dennys Reefs of the Klerksdorp Goldeld, the Steyn, Leader, A and B Reefs of the Welkom Goldeld, and the Carbon Leader Reef of the Carletonville Goldeld. In some polished thin sections, up to 30% of the total uid inclusions contain liquid hydrocarbons. Non-mineralized sandstones and conglomerate lags distal to the mineralized conglomerates also contain oil-bearing uid inclusions, but they are comparatively less abundant. The implication is that the reef horizons were the principal, but not sole, pathways for early oil migration. Furthermore, their larger average grain sizes and higher porosities may well have made reef horizons more susceptible to point-contact fracturing during physical compaction (Zhang et al. 1990), thereby providing more sites for oil entrapment during early burial. Samples examined from the Ventersdorp Contact Reef contain two populations of oil-bearing uid inclusions. The rst population comprises small (<4 m) three-phase inclu- sions. The oil phase appears as a ne clear lm with a dull-white uorescence under UV illumination. The timing of the microfractures which host the liquid hydrocarbons is poorly constrained, but they appear to be Type 2 or Type 4. Oil-bearing uid inclusions of the second population, which are present in only trace amounts, have uorescence features similar to those of oil-bearing uid inclusions from the Witwatersrand Supergroup. It is possible that this second population of oil-bearing uid inclusions is inherited (Type 1). The youngest sedimentary rocks examined in this study are from the Black Reef. Samples from the Carletonville Goldeld and the Potchefstroom Gap Area contain oil in Types 2 and 3 entrapment sites, which is consistent with observations recorded by Dutkiewicz et al. (1998). Oil generation and migration There are several lines of evidence that indicate that oil generation and migration within the Witwatersrand Supergroup can be compared to oil generation and migration in Phanerozoic successions. These include: (i) the presence of suitable source rocks; (ii) evidence for suitable temperature and burial conditions required for source-rock maturation; (iii) evidence of oil and gas trapped in uid inclusions, thus providing direct evidence of hydrocarbon migration; (iv) the presence of bituminous nodules, which record the residual products of hydrocarbon migration. The following section explores this comparison. Source rocks Recent studies suggest that hydrocarbons were most likely sourced from organic matter within shales of the Witwatersrand Supergroup (Law et al. 1991; Gray et al. 1998; Phillips & Law 2000; Spangenberg & Frimmel 2001). Numer- ous thick shales units have been identied (Fig. 6), particularly in the West Rand Group, that contain carbonaceous matter of interpreted primary origin (Gray et al. 1998; Preston & Stevens 1998). Analyses by Gray et al. (1998) indicate post-mature total organic carbon (TOC) levels of up to 1% in shales from the West Rand and Central Rand Groups, which suggests that those rocks would have been adequate petroleum sources. Shales from the Chuniespoort Group of the lower Transvaal Supergroup (Meyer & Robb 1996), and possibly also organic- rich units in the underlying Wolkberg Group (Button 1976), could have been local sources for oil preserved in conglomerate units of the Black Reef. Source rock maturation Oil generation is limited typically to a narrow window of approximately 100-150 C, with source rock maturation generally inuenced by depths of burial and the geothermal gradient of the host basin (Mackenzie & Quigley 1988). For Precambrian basins such as the Witwatersrand, there is some diculty in reconstructing thermal histories because: (i) there is a general lack of the maturity indicators used for Phanerozoic basins, for example, pollen colouration, vitrinite reectance, oil chemistry and/or AFTA measurements (Duddy et al. 1994) and (ii) mudrock sources are normally thermally overprinted by metamorphism. Problems also exist in estimat- ing the burial history of the Witwatersrand Basin because of poor geochronological constraints and lack of estimates of the amount of stratigraphic section removed below unconformities (see Winter 1987). The geothermal gradient of the Witwatersrand Basin prior to the development of the Ventersdorp Supergroup is con- sidered to have been similar to the Rocky Mountains and East Venezuelan Foreland Basins, which have typical values of c.15-35 C km -1 (Tissot & Welte 1984: Osadetz et al. 1992). These values are consistent with previous estimates of the geothermal gradient of the Witwatersrand Basin (Gibson et al. 1997; Jones 1988; Martini 1992), as well as values derived from uid-inclusion analyses (Frimmel et al. 1993). From a combination of even the most-modest geothermal gradients of 15-16 C km -1 (Jones 1988; Martini 1992) and current average thicknesses of the succession (Fig. 7), it is likely that oil generation commenced during deposition of the Central Rand Group, with oil sourced from the lower West Rand Group (Fig. 7). The presence of Types 1 and 2 (Fig. 2) oil inclusions in conglomerates of the Inner Basin Reef (upper West Rand Group) implies that oil migration occurred even earlier. With potential shale sources at various horizons throughout the West Rand and Central Rand Groups, the Witwatersrand Supergroup probably passed progressively through the oil window during burial (Fig. 7). It is likely that source rocks in the Central Rand Group (e.g., Booysens Shale) produced oil during deposition of the Ventersdorp Supergroup, when high geothermal gradients were associated with lithospheric extension and ood-basalt emplacement (Coward et al. 1995). Oil generation within the Witwatersrand Supergroup occurred up to a maximum of 200 million years after ARCHAEAN OIL MIGRATION IN SOUTH AFRICA 197 deposition of the source rocks, thus falling well within the time frame of hydrocarbon systems in Phanerozoic foreland basins (Erlich & Barrett 1992; Osadetz et al. 1992). Such an interpretation is in conict with the suggestion by Robb et al. (1997) that oil generation and migration from Witwatersrand shales occurred at c. 2300 Ma. It is conceivable that by that time, which was at least 400 million years after Witwatersrand deposition, most of the source rocks were outside the oil window (Fig. 7) and probably near the limits of gas generation (c. 230 C, Tissot & Welte 1984), particularly given the post- Witwatersrand tectonic history of the Kaapvaal Craton. Furthermore, the quoted age of c. 2300 Ma, which is derived from UPb dating of uraniferous bituminous nodules in Witwatersrand conglomerates (Robb et al. 1994), may record uranium remobilization (Schidlowski 1981) rather than oil migration and the formation age of bituminous nodules. Oil migration The presence of oil-bearing uid inclusions provides direct evidence that oil migration took place in the Witwatersrand Supergroup. Their locations in compaction related micro- fractures (Type 2) and in early syntaxial quartz overgrowths (Type 3) have Phanerozoic analogues (Lisk & Eadington 1994; Parnell et al. 1998), and imply the presence of oil in formation uids during early burial. The stratigraphic distribution of oil-bearing uid inclusions also indicates that hydrocarbon generation and migration were most likely ongoing throughout basin development, and is consistent with progressive sedi- mentary compaction and kerogen maturation. Although oil- bearing uid inclusions are most abundant in the ore horizons, their presence in non-mineralized conglomerates and sand- stones indicates that oil migration was not conned to the reefs but was basin-wide. In the majority of samples examined from the Witwatersrand Supergroup, there is more than one population of oil-inclusions. This is apparent not only from oil that was entrapped at various stages of the quartz paragenetic sequence (Fig. 2), but possibly also from the variety of dierent coloured inclusions that were entrapped in the same textural sites. In Phanerozoic basins, this multiplicity in oil-inclusions may indicate multiple phases of oil migration or dierent sources of oil (McLimans 1987; Eadington et al. 1991; Parnell et al. 1998). In the case where oil is entrapped in microfractures, inclusions of various oil compositions are entrapped progressively as the fractures slowly heal. It is evident, from even the most oil- saturated siliciclastic reservoirs in Phanerozoic successions, that water will remain the wetting phase, thereby enabling quartz cementation and the trapping of oil inclusions to continue slowly (Lisk & Eadington 1994). As discussed above, the signicance of the variation in uorescence (or, more precisely, oil composition) from Witwatersrand samples is still unclear. Nevertheless, by analogy to several Phanerozoic examples (McLimans 1987; Stasiuk & Snowdon 1997), Witwatersrand sandstones and conglomerates may have received multiple charges of oil of varying composition during burial, as a consequence of changes in oil maturation or oil fractionation during migration. As primary porosity diminishes due to quartz cementation and pressure solution during increasing depth and temperature (Leder & Park 1986), oil migration or entrapment becomes restricted to secondary porosity (e.g., fractures). With evidence for several deformation events during the post-depositional history of the Witwatersrand Supergroup (Coward et al. 1995; Frimmel 1997), the absolute timing of many of the late fractures (Type 4) and veins (Type 5) is dicult to constrain. Only a few of the recognized late fractures (Type 4) contain oil-bearing uid inclusions. However, previous uid inclusion studies (see review in Klemd 1999) have shown that light hydrocarbons (e.g., CH 4 and C 2 H 6 ) and bitumen (e.g., Drennan et al. 1999; Gartz & Frimmel 1999) are present in primary and secondary uid inclusions entrapped in quartz veins. The hydrocarbon gases entrapped in late paragenetic sites may reect increasing maturation levels during later periods of basin evolution, with associated increases in temperatures and burial depths (Fig. 7). Summary and implications for the goldbitumen relationship Oil preserved in uid inclusions within the Witwatersrand Supergroup indicates that there was hydrocarbon generation and migration during the Archaean. Oil-bearing uid inclu- sions are recorded in polished thin-sections of conglomerates and, to a lesser degree, sandstones taken from samples throughout the Central Rand Group, as well as from repre- sentative samples of the upper West Rand Group, the Ventersdorp Contact Reef at the base of the Ventersdorp Supergroup, and the Black Reef at the base of the Transvaal Supergroup. The presence of those oil-bearing uid inclusions in healed microfractures, which developed in detrital quartz Fig. 7. Comparison of the various burial depths required for the onset of oil generation, dependent on the given geothermal gradient applied (1; 15-16 C km -1 ; Jones 1988; Martini 1992; 2 & 4, Frimmel et al. 1993; 3 Gibson et al., 1997) and a sequence thickness of approximately 7 km. It appears, from the diagram, that oil was most likely generated from lower West Rand Group mudrocks prior to the end of deposition of the Central Rand Group. V, Ventersdorp Supergroup; CR, Central Rand Group; WR, West Rand Group. 198 G. L. ENGLAND ET AL. grains during physical compaction, and in early syntaxial quartz overgrowths indicates that the onset of oil mi- gration coincided with early stages of sedimentary burial, when intra-granular porosity was still preserved. This investigation points strongly to the evolution of multiple generations of oil. Evidence includes: (i) that oil was trapped in inclusions in the same type of early diagenetic fabrics throughout the stratigraphic successions; (ii) that many of the oil entrapment sites contain more than one type of oil, as indicated by the variation in UV-uorescent colours (cf. McLimans 1987); (iii) that oil was typically entrapped at multiple stages of the quartz paragenetic sequence that can be identied within single polished thin-sections. It is likely that oil preserved within sandstones and conglomerates of the Central Rand Group and the Ventersdorp Contact Reef was derived from multiple source areas. The lack of oil-bearing uid inclusions, and only the rare occurrence of residual hydrocarbon in the Dominion Reef, imply that the major oil source-rocks were stratigraphically higher than the Dominion Group. This study indicates that oil generation and migration were ongoing throughout and after development of the Witwatersrand Basin, consistent with progressive burial and kerogen maturation. Liquid hydrocarbon identied in uid inclusions from the Black Reef was probably derived from a source other than the Witwatersrand Supergroup, such as carbonaceous mudrocks within the same succession, carbonaceous mudrocks within the overlying Chuniespoort Group, or carbonaceous shales within the underlying Wolkberg Group. The results from this study are in conict with the suggestion by Robb et al. (1997) that onset of oil generation and migration in the Witwatersrand Supergroup occurred at c. 2300 Ma, at some stage during deposition of the Transvaal Supergroup. Analogy with Phanerozoic successions implies that at a similar stage of basin evolution (i.e. at least 400 million years after deposition), source rocks in the Witwatersrand Supergroup were unlikely to be still producing oil and may have already reached the limits of gas generation as the consequence of increasing depth of burial, increasing temperature, and the impact of successive tectonic events. Early oil generation and migration can explain why only a limited number of fractures that developed during late-stage deformation contain oil, and why light hydrocarbons, such as methane, are present in uid inclusions that are hosted in late authigenic quartz and secondary trails in late quartz veins (Drennan et al. 1999; Frimmel et al. 1999). The presence of oil during diagenesis has important impli- cations for the origin of bituminous nodules within the Witwatersrand Supergroup. If rounded uraninite grains represent former detrital heavy minerals, as many petro- graphic studies have proposed (Ramdohr 1958; Minter 1978; Schidlowski 1981), then oil migrating through primary porosity during early stages of burial would almost certainly have been radiogenically immobilized to form bituminous nodules. A similar mechanism for bituminous nodule forma- tion during diagenesis has been established from Phanerozoic depositional basins (Rasmussen et al. 1989, 1993; England et al. 2001), where detrital grains of monazite, xenotime and high-U zircon are enveloped in bitumen that is the residual product of immobilized hydrocarbons. The well-documented occurrence of a signicant proportion of Witwatersrand gold in or adjacent to bitumen seams or nodules (e.g., Pretorius 1991) implies that either detrital gold was remobilized or hydrothermal gold introduced after initial radiogenic immobilization of oil. The timing of this event, which controlled the present siting of most of the gold, was probably late in basin history (i.e., post-Witwatersrand deposition) when (i) primary porosity and permeability in the Central Rand Group were limited, (ii) oil migration was at a minimum and (iii) light hydrocarbons were the primary oil phase. The combination of these factors limited the nature of auriferous uids, if any, that could have deposited gold in zones of structurally induced permeability. 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